The dura mater is the final barrier against cerebrospinal fluid leakage and plays a crucial role in protecting and supporting the brain and spinal cord. Head trauma, tumor resection and other traumas damage it, requiring artificial dura mater for repair. However, surgical tears are often unavoidable. To address these issues, the ideal artificial dura mater should have biocompatibility, anti‐leakage, and self‐healing properties. Herein, this work has used biocompatible polycaprolactone diol as the soft segment and introduced dynamic disulfide bonds into the hard segment, achieving a multifunctional polyurethane (LSPU‐2), which integrated the above mentioned properties required in surgery. In particular, LSPU‐2 matches the mechanical properties of the dura mater and the biocompatibility tests with neuronal cells demonstrate extremely low cytotoxicity and do not cause any negative skin lesions. In addition, the anti‐leakage properties of the LSPU‐2 are confirmed by the water permeability tester and the 900 mm H2O static pressure test with artificial cerebrospinal fluid. Due to the disulfide bond exchange and molecular chain mobility, LSPU‐2 could be completely self‐healed within 115 min at human body temperature. Thus, LSPU‐2 comprises one of the most promising potential artificial dura materials, which is essential for the advancement of artificial dura mater and brain surgery.